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Оптика и спектроскопия

Спектры поглощения пробного сигнала и резонансной флуоресценции для излучателей при их взаимодействии с локальным окружением в прозрачных средах

Е.A. Смирнова, Natalia A. Lozing, М. Г. Гладуш, А.В. Наумов

Published Nov 9, 2021• 0 citations
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Abstract

The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.

DOI
10.21883/os.2022.01.51903.36-21

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The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.
The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.
Abstract The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.
The effect of macroscopic parameters of a substance on the optical characteristics of impurity particles is investigated. A generalized control equation is derived for two-level emitters forming an ensemble of optical centers in a transparent dielectric medium. In this equation, the effective values of the acting pump field and the radiative relaxation rate of an optical center are taken into account. The formalism developed here is a completely microscopic approach based on the chain of the Bogoliubov-Born-Green-Kirkwood-Yvon equations for reduced density matrices and correlation operators for material particles and modes of a quantized radiation field. The method used here makes it possible to take into account the effects of individual and collective behavior of emitters, which are associated with the presence of an intermediate medium, consistently without using phenomenological procedures. It is shown that the resultant analytic expression for the effective lifetime of the excited state of an optical center conforms with experimental data.
Numerical simulations of the excitation spectra of resonant fluorescence bound by the dynamic interaction of two different two-level nanoparticles have been performed. We considered the excitation of one of the particles by monochromatic light with a frequency close to the transition frequency of this particle, at an irradiation intensity leading to a small population of its excited state. The formalism for the description of resonance fluorescence by the Heitler--Ma method was applied to a complete compound system of the marked particle pair and quantized emission field. The resulting expressions for the excitation spectrum reflect consideration of the absorption of the fluorescence photon without attributing it to the emission of any one particle. Expressions for the excitation spectra when taking into account such absorption of the fluorescence photon that allows us to attribute it to the radiation of one or another of the particles were obtained by solving a modified system of equations of the Heitler--Ma method, which reflects the addition of non-interfering amplitudes of the emission field states of each particle. It was found that the shape of the excitation spectra of the stationary resonance fluorescence of the particles in question is determined by the shape of the corresponding intensity spectra of the spontaneous fluorescence of these particles. Keywords: mathematical modeling, interacting two-level nanoparticles, resonant fluorescence, excitation spectrum.
A method is introduced to calculate for a model set of molecular levels the spectral line shapes expected for a variety of conventional laser experiments including absorption, hole burning, fluorescence line narrowing, and Raman scattering. The method allows the incident laser field to have arbitrary intensity. Furthermore, the effects of model Gaussian or Lorenzian inhomogeneous distributions are readily incorporated. Earlier results for a two-level system are easily obtained and new results are presented for inhomogeneously broadened two and three level systems, and for the effects of pure dephasing on the strong field spectra. In particular we have described the differences between fluorescence and Raman in strong fields, and the effect of strong fields on the spontaneous emission of inhomogeneously broadened transitions. Some predictions are made regarding line narrowing experiments in the strong-field limit.